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Sharp, Michael A.

Publications and source records attributed to Sharp, Michael A..

Molybdenum and Tungsten isotope compositions of UO 2 fuel pellets: Implications for isotopically enriched taggants

The addition of isotopically enriched taggants to material at the front end of the nuclear fuel cycle could be a powerful tool used to assist law enforcement authorities should material outside of regulatory control be found. Two potential candidates for this purpose are molybdenum (Mo) and tungsten (W) as both elements have five or more stable isotopes and are trace elements contained within nuclear fuel. So there is a concern that Mo and W could undergo isotope fractionation during processes like uranium enrichment and to date, it is unknown if nuclear fuels have natural Mo and W isotope compositions. If Mo and W isotopic variability is present in nuclear fuels, this would hinder the use of these elements as isotopic taggants because it would be difficult to discern the original taggant isotope composition with high confidence. Therefore, a set of 16 low enriched uranium (LEU) fuel pellets from US commercial producers was analyzed using multi collector-inductively coupled plasma mass spectrometry (MC-ICPMS) to determine Mo and W isotope compositions (i.e., 94 Mo/ 92 Mo, 95 Mo/ 92 Mo, 96 Mo/ 92 Mo, 97 Mo/ 92 Mo, 98 Mo/ 92 Mo, 183 W/ 182 W, 184 W/ 182 W, and 186 W/ 182 W). Relative to terrestrial standards, LEU fuel pellets have variable Mo and W isotope compositions, thereby complicating the use of these elements as isotopically enriched taggants. As such, this work demonstrates that the isotope composition of any potential taggant must be well characterized in the base nuclear fuel prior to any taggant addition. Furthermore, these results suggest that Mo and W are not ideal candidates for isotopically enriched taggants.

58 GEOSCIENCES↗

Collaborative Study for Certification of Trace Elements in Uranium Ore Concentrate CRMs UCLO-1, UCHI-1, and UPER-1

Trace impurity patterns are important nuclear forensic signatures in uranium ore concentrates (UOCs) and Certified Reference Materials (CRMs) are used to validate the analysis methods employed by end users. Herein, we discuss the certification campaign for three new UOC CRMs from the National Research Council Canada: UCLO-1 (https://doi.org/10.4224/crm.2020.uclo-1), UCHI-1 (https://doi.org/10.4224/crm.2020.uchi-1), and UPER-1 (https://doi.org/10.4224/crm.2020.uper-1). This study involved 15 laboratories from 10 countries, using sector-field and (triple) quadrupole inductively-coupled plasma mass spectrometry to analyze 64 trace element impurities. We discuss the importance of the acids used for sample digestion, difficulties analyzing in a high uranium matrix, and data combination and uncertainty evaluation for this large dataset.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Exploring the use of thorium isotope compositions and concentrations as nuclear forensic signatures for uranium ore concentrates

This interlaboratory study measured thorium concentrations and isotope compositions in uranium ore concentrates from different geographical locations to examine whether thorium impurities may be useful forensic signatures for uranium ore concentrates found out of regulatory control. Measured 230 Th/ 232 Th in fifteen uranium ore concentrates record over three orders of magnitude of compositional variation. Results demonstrate that 230 Th/ 232 Th used in combination with U/Th ratios resulted in a unique signature for individual uranium ore concentrates from different processing locations. Data presented here suggest potential for 230 Th/ 232 Th and U/Th to be used as comparative signatures to investigate the provenance of seized uranium ore concentrates.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Samarium isotope compositions of uranium ore concentrates: A novel nuclear forensic signature

Uranium ore is mined and milled to produce uranium ore concentrate (UOC), a regulated product of the nuclear fuel cycle. Additionally, diversion of UOC from the fuel cycle into possible weapons production is a key concern in global nonproliferation efforts. As such, the ability to trace the origin of seized nuclear materials is imperative to law enforcement efforts. Although isotopic signatures of UOCs have proven fruitful to pinpoint sample provenance, new isotopic signatures are needed because most existing isotopic signatures are not indicative of the original ore body from which the U is derived. In this work, we developed a new method to separate samarium (Sm) from a U-rich sample matrix and report the first Sm isotope compositions of 32 UOCs derived from a variety of worldwide uranium mines. Relative to terrestrial standards, approximately half the UOCs have resolved and anticorrelated 149 Sm- 150 Sm isotope compositions, consistent with the capture of thermal neutrons by 149 Sm in the ore body. The UOCs with anomalous Sm isotope compositions tend to derive from older (~>1.5Ga) and higher-grade ore bodies, although other factors, such as the presence of neutron moderators like water, also play a role. Nonetheless, the Sm isotope compositions of UOCs directly reflects the neutron fluence over the history of the original ore body and can be used to discern different geologic conditions associated with that ore body. Overall, this work demonstrates the potential use of Sm isotopes as a novel nuclear forensics signature for origin assessment of UOCs.

58 GEOSCIENCES↗